论文标题
Ruddlesden-Popper Halide perovskites与八面体旋转的Rashba-/dresselhaus效应的出现
Emergence of Rashba-/Dresselhaus Effects in Ruddlesden-Popper Halide Perovskites with Octahedral Rotations
论文作者
论文摘要
Ruddelsden-Popper Halide Perovskites是高度用途的准二维能量材料,具有广泛的可调光电特性。 Here we use the all-inorganic Cs$_{n+1}$Pb$_n$X$_{3n+1}$ Ruddelsden-Popper perovskites with X=I, Br, and Cl to systematically model the effect of octahedral tilting distortions on the energy landscape, band gaps, macroscopic polarization, and the emergence of Rashba-/Dresselhaus splitting in these 材料。我们构建了所有独特的$ n = 1 $和$ n = 2 $结构,从八面体倾斜到结构,并使用第一原理密度功能理论来计算总能量,极化和频段结构,并使用$ GW $近的频带隙计算来备份。我们的结果为通过振幅,方向和化学特征的相互作用的抗毒性变形模式的幅度,方向和化学特征的相互作用提供了设计规则,以定制结构扭曲和谱势特性。我们的工作强调,与3D钙钛矿相比,极性结构可能是由八面体倾斜的组合以及这类材料中的rashba-/dresselhaus分裂而产生的,这是由极性失真模式的方向和PB-1轨道贡献确定的。
Ruddelsden-Popper halide perovskites are highly versatile quasi-two-dimensional energy materials with a wide range of tunable optoelectronic properties. Here we use the all-inorganic Cs$_{n+1}$Pb$_n$X$_{3n+1}$ Ruddelsden-Popper perovskites with X=I, Br, and Cl to systematically model the effect of octahedral tilting distortions on the energy landscape, band gaps, macroscopic polarization, and the emergence of Rashba-/Dresselhaus splitting in these materials. We construct all unique $n=1$ and $n=2$ structures following from octahedral tilts and use first-principles density functional theory to calculate total energies, polarizations and band structures, backed up by band gap calculations using the $GW$ approach. Our results provide design rules for tailoring structural distortions and band-structure properties in all-inorganic Ruddelsden-Popper perovskites through the interplay of the amplitude, direction, and chemical character of the antiferrodistortive distortion modes contributing to each octahedral tilt pattern. Our work emphasizes that, in contrast to 3D perovskites, polar structures may arise from a combination of octahedral tilts, and Rashba-/Dresselhaus splitting in this class of materials is determined by the direction and Pb-I orbital contribution of the polar distortion mode.